Cyanide-catalyzed aldimine coupling was employed to synthesize compounds with 1, 2-ene- diamine and α-imine-amine structural motifs: 1, 2, N, N'-tetraphenyletheylene-1, 2-diamine (13) and (±)-2, 3-di-(2-hydroxyphenyl)-1, 2-dihydroquinoxaline (17), respectively. Single- crystal X-ray diffraction provided solid-state structures and density functional theory calculations were used to probe isomeric preferences within this and the related hydroxy- ...